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Results for “Fullerenes”
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Utilizing Essential Symmetry Breaking in Auxiliary-Field Quantum Monte Carlo: Application to the Spin Gaps of the C 36 Fullerene and an Iron Porphyrin Model Complex
We present three distinct examples where phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) can be reliably performed with a single-determinant trial wave function with essential symmetry breaking. Essential symmetry breaking was first introduced by Lee and Head-Gordon [ Phys. Chem. Chem. Phys. 2019, 21, 4763-4778, 10.1039/C8CP07613H]. We utilized essential complex and time-reversal symmetry breaking with ph-AFQMC to compute the triplet–singlet energy gap in the TS12 set. We found statistically better performance of ph-AFQMC with complex-restricted orbitals than with spin-unrestricted orbitals. We then showed the utilization of essential spin symmetry breaking when computing the singlet–triplet gap of a known biradicaloid, C 36 . ph-AFQMC with spin-unrestricted Hartree–Fock (ph-AFQMC+UHF) fails catastrophically even with spin-projection and predicts no biradicaloid character. With approximate Brueckner orbitals obtained from regularized orbital-optimized second-order Møller–Plesset perturbation theory (κ-OOMP2), ph-AFQMC quantitatively captures strong biradicaloid character of C 36 . Lastly, we applied ph-AFQMC to the computation of the quintet–triplet gap in a model iron porphyrin complex where brute-force methods with a small active space fail to capture the triplet ground state. We show unambiguously that neither triplet nor quintet is strongly correlated using UHF, κ-OOMP2, and coupled-cluster with singles and doubles (CCSD) performed on UHF and κ-OOMP2 orbitals. There is no essential symmetry breaking in this problem. By virtue of this, we were able to perform UHF+ph-AFQMC reliably with a cc-pVTZ basis set and predicted a triplet ground state for this model geometry. The largest ph-AFQMC in this work correlated 186 electrons in 956 orbitals. Our work highlights the utility, scalability, and accuracy of ph-AFQMC with a single-determinant trial wave function with essential symmetry breaking for systems mainly dominated by dynamical correlation with little static correlation.
Efficient Charge Generation via Hole Transfer in Dilute Organic Donor–Fullerene Blends
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Synthesis and Stability of Actinium-225 Endohedral Fullerenes, 225 Ac@C 60
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Long-range exciton diffusion in molecular non-fullerene acceptors
Abstract The short exciton diffusion length associated with most classical organic semiconductors used in organic photovoltaics (5-20 nm) imposes severe limits on the maximum size of the donor and acceptor domains within the photoactive layer of the cell. Identifying materials that are able to transport excitons over longer distances can help advancing our understanding and lead to solar cells with higher efficiency. Here, we measure the exciton diffusion length in a wide range of nonfullerene acceptor molecules using two different experimental techniques based on photocurrent and ultrafast spectroscopy measurements. The acceptors exhibit balanced ambipolar charge transport and surprisingly long exciton diffusion lengths in the range of 20 to 47 nm. With the aid of quantum-chemical calculations, we are able to rationalize the exciton dynamics and draw basic chemical design rules, particularly on the importance of the end-group substituent on the crystal packing of nonfullerene acceptors.
Non-fullerene acceptor organic photovoltaics with intrinsic operational lifetimes over 30 years
Abstract Organic photovoltaic cells (OPVs) have the potential of becoming a productive renewable energy technology if the requirements of low cost, high efficiency and prolonged lifetime are simultaneously fulfilled. So far, the remaining unfulfilled promise of this technology is its inadequate operational lifetime. Here, we demonstrate that the instability of NFA solar cells arises primarily from chemical changes at organic/inorganic interfaces bounding the bulk heterojunction active region. Encapsulated devices stabilized by additional protective buffer layers as well as the integration of a simple solution processed ultraviolet filtering layer, maintain 94% of their initial efficiency under simulated, 1 sun intensity, AM1.5 G irradiation for 1900 hours at 55 °C. Accelerated aging is also induced by exposure of light illumination intensities up to 27 suns, and operation temperatures as high as 65 °C. An extrapolated intrinsic lifetime of > 5.6 × 10 4 h is obtained, which is equivalent to 30 years outdoor exposure.
Traps and transport resistance are the next frontiers for stable non-fullerene acceptor solar cells
Stability is one of the most important challenges facing material research for organic solar cells (OSC) on their path to further commercialization. In the high-performance material system PM6:Y6 studied here, we investigate degradation mechanisms of inverted photovoltaic devices. We have identified two distinct degradation pathways: one requires the presence of both illumination and oxygen and features a short-circuit current reduction, the other one is induced thermally and marked by severe losses of open-circuit voltage and fill factor. We focus our investigation on the thermally accelerated degradation. Our findings show that bulk material properties and interfaces remain remarkably stable, however, aging-induced defect state formation in the active layer remains the primary cause of thermal degradation. The increased trap density leads to higher non-radiative recombination, which limits the open-circuit voltage and lowers the charge carrier mobility in the photoactive layer. Furthermore, we find the trap-induced transport resistance to be the major reason for the drop in fill factor. Our results suggest that device lifetimes could be significantly increased by marginally suppressing trap formation, leading to a bright future for OSC.
Interfacial electronic structure of Cl6SubPc non-fullerene acceptors in organic photovoltaics using soft X-ray spectroscopies
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Ferrocene as a highly volatile solid additive in non-fullerene organic solar cells with enhanced photovoltaic performance
Ferrocene was introduced as a solid additive in organic solar cells (OSCs). The use of ferrocene provides PM6:Y6 based device with improved performance and stability, demonstrating its great potential in the fabrication of efficient and stable OSCs.
Transannularly conjugated tetrameric perylene diimide acceptors containing [2.2]paracyclophane for non-fullerene organic solar cells
Two isomeric perylene diimide acceptors with through-space conjugated [2.2]paracyclophane as a central core show dramatic differences in device performances.
Tailoring non-fullerene acceptors using selenium-incorporated heterocycles for organic solar cells with over 16% efficiency
The selenium substitution strategy was applied to develop two new A′-DAD-A′-type small molecular acceptors. The resulting selenium-incorporated molecules exhibit red-shifted absorption and an enhanced photon response, leading to high device efficiencies of over 16%.
Incorporation of alkylthio side chains on benzothiadiazole-based non-fullerene acceptors enables high-performance organic solar cells with over 16% efficiency
This is the first time alkylthio chains are employed on Y6-like NFAs to achieve organic solar cells of power conversion efficiency higher than 16%.